Synthesis of Hydrocarbon Fuels

8/2/2019 Synthesis of Hydrocarbon Fuels

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SYNTHESIS OF HYDROCARBON FUELS USING RENEWABLE AND NUCLEAR ENERGY

Ken Schultz

General Atomics, 3550 General Atomics Court, San Diego, CA 92121, [email protected]

S. Locke Bogart

General Atomics Consultant, 7982 Chaucer Drive, Weeki Wachee, FL 34607, [email protected]

Richard P. Noceti

National Energy Technology Laboratory and LTI Associates, P.O. Box 178, Bannock, OH 43972. [email protected]

In light of the current issues of carbon control and

the desire to become less dependent on imported oil, we

propose to apply non-carbon-based energy supplies

(renewables and nuclear) to reduction of CO2 emissions

and production of liquid synthetic fuels. To this end we

have performed technical and economic analyses of

systems ranging from augmentation of coal-to-liquidsprocesses, through the use of coal power plant CO2 to the

extraction of atmospheric CO2 for the production of

synthetic fuels.

This paper emphasizes the utilization of coal power

plant CO2 and points towards the closure of the carbon

cycle by the ultimate use of atmospheric CO2.

I. INTRODUCTION

Renewable and nuclear energy based production of

synthetic hydrocarbon fuels (synfuels) can help reduce

CO2 emissions and address the growing shortage ofpetroleum. Refined petroleum products and synfuels can

be generically expressed as [CH2]n, where n is

significantly greater than two. Currently, synfuels are

produced from coal and natural gas. With increasing

natural gas prices, there will be a greater emphasis on coal

as a feedstock. In coal-to-liquids (CTL) processes that go

through gasification to synthesis gas [CO + H2], about one

molecule of CO2 is made for every CH2 unit in the

synfuel. Displacing petroleum with coal-based fuels for

our transportation sector can be done in ways that will

reduce CO2 emissions. This investigation explores the

concepts of how renewable and nuclear energy could help

the simultaneous problems of CO2 emissions anddwindling petroleum supplies.

The production rate of CO2 from coal electric power

plants in the US is ~1,894 million metric tons/year. If this

CO2 were captured using proven processes and used with

hydrogen produced by solar, wind or nuclear energy to

make synfuel, it would provide all the hydrocarbon fuel

needed for our transportation sector. This sector emits

~1,891 million metric tons of CO2 per year from

petroleum based fuels which is about one third of the total

US emissions of 5,900 million metric tons per year. Using

this synfuel process would cut our total CO2 production

by one-third. We could shift from petroleum-based

transportation to synfuel-based. This would reduce our

petroleum use by ~75%, and reduce our CO2 production

by ~33% with no sequestration. It would requiresignificant quantities of hydrogen (~255 million metric

tons/year, or 25 times our current production) that could

be produced from splitting of water using solar, wind, or

other renewables or nuclear energy.

In addition to significantly reducing our use of

petroleum, and cutting our CO2 emissions by one-third,

this concept would allow use of our existing hydrocarbon-

based transportation infrastructure.

II. GLOBAL CLIMATE CHANGE & CO2

EMISSIONS

Carbon dioxide emissions from the burning of fossil

fuels are thought to be causal in global climate change. If

this is true, then it is possible to control or slow global

climate change by preventing carbon dioxide from

entering the atmosphere or by removing what has already

been emitted.

We may prevent carbon dioxide from entering the

atmosphere by capturing it at its sources and sequestering

[storing] it. It can be captured and then stored

underground in geologic formations such as deep saline

aquifers or depleted gas fields. [Note that some CO2 is

used for secondary oil recovery. In this process, CO 2 ispumped into an oil field and displaces some of the

residual oil left in the field. This process is not generally

considered to be sequestration.]

Carbon sequestration is a major program within

DOEs Office of Fossil Energy and is now being

practiced in several places. One is in the North Sea gas

fields at the Sleipner Well. The gas being produced has,

as many gas wells do, a significant amount of CO2 in it. In


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the past, such well platforms separated CO2 from the

natural gas and vented it to the atmosphere.About 2,800metric tons of carbon dioxide are separated daily from

Sleipner West's gas production and injected into the

Utsira sandstone formation (aquifer), 3,000 feet beneath

the seabed, for long term storage. While a technical

challenge, this is not as difficult a process as separating

CO2 from a more dilute stream, such as a flue gas from a

conventional pulverized coal power plant, and

compressing, transporting and injecting it.

As a rule of thumb, US carbon dioxide emissions are

about one third from power, one third from transportation,

and the final third from everything else, commonly

referred to as industrial processes. Capturing and

sequestering CO2 from fossil-based power plants would

reduce US carbon emissions by one third. Power plants

provide the best targets for capture and sequestration

because they are significant, stationary, point-sources of

CO2, and have a limited, common set of operations,

making a given capture process easier to accomplish. Incontrast, transportation vehicles would require compact

onboard separation and storage, a technical challenge, and

would need the collection and transport of captured CO2 a

logistical hurdle. The remainder of our emissions, the

everything else category, are from uses that do not have

many operations in common and are more diffuse than

power plants.

One problem with CO2 capture in the existing fleet of

power plants is that they use air to combust the fossil fuel,

mainly coal. Air is about 20% oxygen and 80% nitrogen,

which means that most of the combustion exhaust [flue

gas] is atmospheric nitrogen and, consequently, the CO2 isrelatively dilute. This is burdensome in that it is more

difficult and expensive to remove the CO2 from this

stream. In the future, fossil-based power plants will be

designed to provide concentrated, sequestration-ready

CO2 streams. Some of these advanced plant configurations

are being developed and demonstrated under the DOE

FutureGen initiative and include Integrated Gasification

Combined Cycle plants, chemical looping combustion

processes, and Oxyfuel combustion (implemented, for

example, by Vattenfall at the Schwarze Pumpe facility in

eastern Germany). This last concept separates the air

before combustion and only uses the oxygen, providing a

flue gas that is mostly CO2 and water.

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In practice, someof the exhaust CO2 would be recycled to dilute the oxygen

during combustion to cool the flame to temperatures

similar to existing combustion with air. Note that the

exhaust with this scheme is still mostly CO2 and water.

III. PETROLEUM-BASED FUELS

Although fossil fuels now provide most of the

worlds energy, these fuels will become limited in supply

and more costly. About 40% of the U.S. energy demand is

met by oil that is converted primarily to liquid

transportation fuels (gasoline, diesel, and jet fuel).

Todays transportation system depends upon liquid fuels

because of their high gravimetric and volumetric energy

density and their ease of storage, handling, and transport.

Unfortunately, the world is exhausting its resources (Fig.

1) of the light crude oils used to make liquid fuels, with

consumption of oil exceeding discoveries since 1985.3

Fig. 1. Rate of world discovery and consumption of

conventional crude oils vs. time.

A half-century ago, M. King Hubbert developed a

phenomenological model to forecast the peaking of oil

production in the lower forty-eight of the United States.

This model was principally based on the certainty that the

production of a finite resource, e.g., petroleum, will

follow a family of bell-shaped curves depending on

different initial production rates and estimates of the

ultimate size of the resource. He predicted that the year of

peak US oil production would be about 1970.4

In 1970,

US oil production in fact did peak, confirming theprediction made some fifteen years earlier. According to

more pessimistic sources, about half of the worlds oil has

already been consumed (Fig. 2), while the remaining oil

will be increasingly difficult to recover.5,6

The peak of

the conventional oil supply is predicted to occur in the

near-term. Although other sources predict the peak to

occur later, most predictions vary by only a decade or so.

For a report on this issue commissioned by the U.S.

Department of Energy, see reference 6.

Natural gas can be converted to synthetic liquid

hydrocarbon fuel and is more plentiful than oil but still

limited. The US DOE Energy Information Agency showsUS consumption at 22.3 trillion cubic feet (TCF) per year,

with proven reserves of 198 TCF (9 years worth) and

unproven but expected reserves of 1430 TFC (65 years

worth at the current rate of consumption).7

Increasing

consumption is already pushing prices up and projected

lifetimes down. Coal is plentiful, with supplies said to last

hundreds of years at current rates of consumption, but

there are environmental costs of mining, transporting, and

using coal that must be addressed. Although humankind


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will continue to rely heavily on fossil fuels for its energy

needs for much of this century, the challenge during that

time must be to find and develop acceptable alternatives.

In fact, the U.S. General Accountability Office has

released a document expressing its concern with the

potential for the global peaking of conventional petroleum

production.8

Fig. 2. A prediction of the world oil supply.

IV. SYNTHETIC HYDROCARBON FUELS

SYNFUEL

IV.A. Synfuel by Coal Gasification

Synthetic liquid hydrocarbons have been synthesized

for more than three-quarters of a century from non-liquid

feedstocks principally coal but also natural gas in

recent years. The leading process is the Fischer Tropsch

(F-T) process which uses synthesis gas hydrogen and

carbon monoxide as its feed and produces a clean,

sulfur- and aromatic-free precursor that is readily

processed to a range of commercial finished products

using existing petrochemical operations.9 The synthesis

gas is produced by coal gasification and by reforming of

natural gas. Both of these initial conversion processes (in

addition to the cost of the feed) can represent a significant

cost component of the entire synthesis process. For coal,

synthesis gas is produced according to the net reaction:

2C + 1/2O2

+ H2O 2CO + H

2. The Water-Gas Shift

reaction can be used to produce additional H2: CO + H2O

H2

+ CO2The reaction for producing Fischer-Tropsch

products from synthesis gas (CO and H2) is : CO + 2H

2

CH2

+ H2O. Thus, the simultaneous Fischer-Tropsch and

Water-Gas Shift reactions in the reactor leads directly to

the complete reaction: 2C + H2O + 1/2O2 = CH2 + CO2.Note that two carbons are required to produce one

Fischer-Tropsch CH2

product with the other carbon being

emitted as carbon dioxide.

Gasification C + 1/2O2 + H2O 2CO + H2

Water gas shift CO + H2O H2 + CO2

F-T reaction CO + 2H2 CH2 + H2O

Net reaction 2C + H2O + 1/2O2 CH2 + CO2

It should be noted that the above is the theoretical reaction

scheme. The actual series of reactions is quite complex

but the net result is shown. Note also that the gasification

reaction occurs above 2000 F and the heat for this

reaction comes from partial combustion of the

carbonaceous feed, be it coal, biomass, or natural gas.

This reduces the amount of carbon used to reduce water

and increases CO2 production.

IV.B. Synfuel by Coal Gasification + Hydrogen from

Water-splitting

The extra hydrogen that is provided by the Water-

Gas Shift can be provided by splitting of water with

energy supplied from a non-CO2-emitting source. In this

case, we still provide synthesis gas as above: C + 1/4O2

+

1/2H2O CO + 1/2H

2and then provide the extra

hydrogen by water-splitting: 3/2H2O = 3/2H

2+ 3/4O

2, for

a net reaction of C + H2O + Energy CH2 + 1/2O2.

Gasification C + 1/4O2 + 1/2H2O CO + 1/2H2

Water-splitting 3/2H2O + Energy 3/2H2 + 3/4O2


Net reaction C + H2O + Energy CH2 + 1/2O2

In comparison with the conventional gasification and

Fischer-Tropsch sequence, only half the carbon is

required, and there is no CO2 produced in the conversion

process other than the smaller fraction necessary for

reaction heat. Further, oxygen is provided by the water-

splitting, which avoids the need for an air separation unit

for the gasification process, and even has some excessoxygen for potential sale.

IV.C. Synfuel by CO2 Capture + H2 from Water-

splitting

Fossil-fired power plants produce CO2 which could

be captured and converted to CO for production of

synthetic fuels. CO2 can be converted to CO by the

Reverse Water Gas Shift Reaction, CO2 + H2 CO +

H2O. CO could then be used in the F-T reaction with

additional hydrogen from water-splitting to produce

synfuel. Recent studies using novel reaction schemes,

such as membrane reactors, show promise for facile

Water-Gas Shift and Reverse Water Gas Shift

conversions.10

Reverse Water Gas Shift CO2 + H2 CO + H2O


Water-splitting 3H2O + Energy 3H2 + 3/2O2

Net reaction CO2 + H2O + Energy CH2 + 3/2O2


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In this case, only the coal used to produce power is

needed, and the resulting CO2 is consumed rather than

released. The excess O2 would be used as Oxyfuel in the

fossil power plant that provides the CO2, simplifying CO2

capture. Figure 3 illustrates the complete block diagram

for an idealized process.

Fig. 3. Oxyfuel Coal Plant and Fischer-Tropsch ProcessesAugmented with Externally Provided Oxygen and

Hydrogen Produced by Water-Splitting.

There is currently considerable effort underway on

developing CO2 capture systems for new and extant

power plants. In previous papers, we have discussed

Membrane Gas Absorption approaches for retrofitting

existing coal power plants for post-combustion CO2

capture11,12

and this material will not be reproduced here.

Rather we will focus on the Oxyfuel configuration as

shown in Figure 3 as there is reasonable optimism that

some existing pulverized coal (PC) plants may be

retrofittable because of the considerably smaller gas-flow

due to the absence of nitrogen.

Such a synergistic system, as described above,

dubbed twice burned coal or recycled coal, has the

potential to significantly reduce our current emissions of

CO2 since the carbon in the coal is used once for power

production and then again for liquid hydrocarbon fuel

synthesis. Fig. 4 illustrates the Crystal River plant, owned

and operated by Progress Energy, that has four PC plants

rated at 2,313 MWe, total and one nuclear plant rated at

838 MWe. For the twice-burned coal case, there would be

one Oxyfueled plant rated at ~ 400 MWe net output and

two nuclear plants rated at ~ 2,270 MWe (total) for fuel

production. This plant would produce ~ 790,800 gallonsper day of motor fuel. Serendipitously, this would be the

demand of each energy form for about 200,000

households.

Fig. 4. The Progress Energy Crystal River Facility with 4

Pulverized Coal Plants and 1 Nuclear Plant.

V. ECONOMIC ESTIMATES

While the concept of using an external source of

hydrogen to reduce or even eliminate CO2 production

while making synfuel is exciting, the economics have to

be reasonable. We did some simple analyses to explore

the economics.

TABLE 1 400 MWe Oxyfuel Plant Cost Basis and COE

For the Oxyfueled PC plant, we used the cost basis

presented by the Department of Energys National Energy

Technology Laboratory13

and reproduced above, in Table

1, with the ASU and the CO2 compressor costs and power


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requirements eliminated. Because of this, the COE isvirtually identical to that associated with a PC plant thatrejects its CO2 into the atmosphere. However, in this case,the synfuel plant takes all of the CO 2 and converts it totransportation fuel. Note the levelizing factors in the table(17.9 % for current $ and 14.8% for constant $) aretypical for an investor-owned utility. Below, we will lookat this in terms of the cost of capital for Public and Privatesector investment.

Previous work on the hydrogen-assisted CTLprocess, briefly discussed in section IV.A., was based ona scoping study performed by Rentech for the state ofWyoming for synthetic diesel fuel and electricityproduction from Powder River Basin coal using coalgasification and the Fischer-Tropsch synthesis process.14For their baseline economic assumptions, they estimatethe cost of synfuel production, including both capital andoperating costs, at $0.95/gallon. The baseline assumptionsinclude coal at $5.00/ton and a 6.5% cost of capital.

Adjusting these to more realistic values of $30/ton forcoal and 10% (Public Sector) interest raises the cost ofsynfuel to ~$1.85/gallon, still a reasonable cost. However,this plant would emit to the atmosphere about 20 kg ofCO2 for each gallon of fuel it is to produce. Should thiscost be internalized, it would amount to ~$0.60 pergallon.

For this analysis, we adopted the cost figures thatwere offered in the Rentech presentation only for theFischer-Tropsch part of their plant as the remainder of theplant is related to coal processing and electricityproduction. We further assumed that a reverse water gas

shift reaction system would have approximately the samecost characteristics as the F-T component since thevolumetric flow rates and thermodynamic properties aresimilar. We then estimated the benefit of getting theoxygen and hydrogen needed for the entire process fromnuclear power (the baseline carbon-free sustainableenergy technology we selected for this analysis).

The cost of the oxygen and hydrogen was estimatedfor production using the Sulfur-Iodine thermochemicalwater-splitting process coupled to the Modular HeliumReactor, 15 and also for production by standard lowtemperature electrolysis using electricity from a Light

Water Reactor. Table 2 presents the results of thisanalysis for two Capital Recovery Factors (10% and 15%)and Nominal & Low plant costs (for the electrolyserefficiency, Nominal is 54.7 kWh/kg of H2 and Low is49.2 kWh/kg of H2).

TABLE 2. Estimated Cost of Synfuel, $/gallon(without/with $30/tonne CO2 Consumption credit; withAdditional $30/tonne Avoided CO2 Credit With Respectto the Rentech Plant).

Consider first the effect of the Interest Rate (FixedCharge Rate or Capital Carrying Charge in Table 2). Theeffect of the Carrying Charge on the cost of the fuelproduct is striking, especially for the highest capital costplant (Nominal LWR plant). Even for the lowest capitalcost plant (Low HTR), it is still significant. Consequently,for economic competitiveness, it is very desirable to fundsuch a plant as a Public/Private enterprise in order toobtain the lowest possible capital charge. There are bothlarge and small scale examples of such partnerships thatspan the range from a TVA to a multiplicity ofMunicipal utilities.

Next, it is important to note that the cost of the

hydrogen/oxygen production system dominates the capitalcost. This is not surprising as both hydrogen and highquality thermal/electrical technologies are expensive. It isespecially noted that there is considerable incentive toreduce the cost and increase the efficiency of electrolysersystems for nearer-term deployment.

It is almost a given now that the costs associatedwith reducing (consuming) CO2 emissions will be


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internalized in the next few years. So, the rows of datathat reduce the raw cost by the $30/Tonne of CO2 arerealistic. How this charge eventually will be internalizedis still uncertain. Should it be a tax to penalize CO2emitters rather than a credit given as offsets (tradable in amarket), then these cost reductions may not materialize.However, then the cost of coal-based synfuel would risean equivalent amount.

In addition there is the interesting discussioncontaining further cost reductions called Avoided CO2. Inthis case, we use as a baseline the Rentech plant discussedabove and compare our system to it. The justification isthat the Rentech plant is what one would build today ifCTL plants had to be built. Comparing the plant typesside by side, we see that the Rentech plant is a netproducer of CO2 (~ 20 kg/gal) and our plant is a netconsumer of CO2 (~ 9.6 kg/gal). While it is not clear thatsuch a credit might be taken, it draws a very compellingdistinction between the two concepts.

Finally, it is worth noting the rows of costs in 10%FCR / CO2 Consumption case. It is very reasonable toassume that tenth-of-a-kind plant capital costs will lie inthe Low cost range. Should this be the case, then theLWR system and HTR systems would produce fuels verylikely below $2.00 per gallon.

VI. SYSTEMS ANALYSIS

The overall impact of alternative sources oftransportation fuels can be seen by examining the CO2flows resulting from energy consumption.16 Our current

total US emission is 5,682 million metric tonnes(MMt)/yr. Our petroleum-based transportation economyreleases 1,811 MMt of CO2 per year. Approximatelyanother 100 MMt of CO2 are released in the productionand processing of that petroleum for at total of 1911MMt/yr. See Table 3.

If this petroleum based transportation economy werereplaced by a coal-based economy using coal gasificationand Fischer-Tropsh conversion, the consumption of coalwould be tripled to 1678 MMt/ year of C as coal, and theproduction of CO2 from transportation doubled to 3857MMt/yr.

If a CO2-free source of hydrogen, such as nuclear orsolar energy, is provided, production of synfuels could bedone using 556 MMt/yr of carbon as coal and producing1,905 MMt/yr of CO2. This would mean doubling ourcurrent consumption of coal but with no increase in ourcurrent production of CO2 as the coal based fuels woulddisplace petroleum. If the carbon needed for synfuel wereprovided from CO2 captured from flue gas of our currentcoal-fired power plants (the focus of this paper), the mass

flows match well. About 565 MMt/yr of carbon is usedand released in the form of CO2, and about 565 MMt/yr isneeded for synfuel production. We could provide all ofour transportation fuel using CO2 captured from ourcurrent coal-fired power plants. This would require noadditional coal use and would actually cut our currentrelease of CO

2by one-third. Both these scenarios would

require a significant increase in the amount of hydrogenthat would have to be produced, and would requiredevelopment of non-CO2 emitting techniques, such ascommercial water splitting, for its production. Thesealternate scenarios are summarized on Table 3.

TABLE 3. Fuel Needed and CO2 Released for AlternateTransportation Fuel Sources

Transportation Fuel From

Units: MMt/yrOil Coal Coal +

H2fromwater

CO2 +H2

fromwater

Oil needed 612 -- -- --Coal needed -- 1113 556 0

H2 needed -- -- 130 260

CO2 produced ~100 2046 104 -1811

CO2 released onuse

1811 1811 1811 1811

Net CO2 released 1911 3857 1905 0

Current total CO2 production: 5,682 MMt/yrCurrent C as coal use/CO2 produced: 565/2070MMt/yr, H2 use: 10 MMt/yr

VII. CONCLUSIONS

Production of synthetic hydrocarbon fuels can helpwith our growing dependence on declining petroleum. Inproduction of synfuels from coal, one atom of carbon isproduced as CO2 for every atom produced as CH2 in thesynfuel. If hydrogen is provided from an external, non-fossil source, such as solar, wind or nuclear production ofhydrogen from water, the synfuel production process neednot produce any CO2. However, the synfuel, when burnedfor transportation will produce and release the containedcarbon as CO2. Since the synfuel would be a replacementfor petroleum-based fuel, there would be no net increasein the production or release of CO2. If the hydrogen isprovided from an external, non-fossil source, and if the

carbon is provided by capture of CO2 from existing coal-fired power plants, the total U.S. release of CO2 can bereduced by one-third. Hydrogen would be used toproduce CO from CO2 in the reverse water gas shiftreaction and to produce [CH2]n from CO and H2 in theFischer-Tropsch reaction. Three molecules of H2 wouldbe needed for every moiety of CH2 produced.


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The production rate of CO2 from coal power plants in

the US is 1,891 million metric tons/year. If this CO2 were

captured using proven extraction processes and used with

hydrogen produced by solar, wind or nuclear energy to

make synfuel, it would provide all the hydrocarbon fuel

needed for our transportation sector. Since transportation

produces 1,911 million metric tons of CO2

per year, this

synfuel process would cut our CO2 production by one-

third while still using our existing hydrocarbon-based

transportation infrastructure. We could shift from a

petroleum-based transportation sector to a synfuel-based

transportation sector. This would reduce our petroleum

use by 75%, and reduce our CO2 production by 33%. It

would require significant quantities of hydrogen (260

million metric tons/year, or 25 times our current

production) that would be produced from water using

solar, wind or nuclear energy.

Our economics estimates indicate that use of

hydrogen in the synfuel production process from power

plant CO2 capture appears to be practical and may berequired to help mitigate climate change, and would allow

synfuel to be produced with only minor cost increase over

coal-based synfuel production.

Earlier work (references 11 and 12) revealed the

further potential for the production of synthetic fuel with

CO2 extracted from the atmosphere which is envisioned to

be the longer-term goal of our current research. The

hydrogen production infrastructure needed for synfuel

production could also be used to produce hydrogen for

direct application via fuel cells in the future. A hydrogen-

synfuel economy could provide a bridge to a future pure

hydrogen economy.

ACKNOWLEDGMENTS

This work was supported by General Atomics

internal R&D funds.

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Synthesis of Hydrocarbon Fuels

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